Magnetoelastic coupling across competing ferromagnetic and ferrimagnetic orders in -site-disordered
Phys. Rev. B 114, 094408 – Published 4 August, 2026
DOI: https://doi.org/10.1103/qjn8-rfhl
Abstract
We show that the magnetic ground state of the double perovskite is jointly controlled by -site (Nd/Sm) mixing, -site (Ni/Mn) ordering, and spin-lattice coupling, with the rare-earth sublattice actively participating in the low-energy magnetic balance. Synchrotron x-ray diffraction (SXRD) and Rietveld refinement establish a monoclinic () structure with predominant -site rocksalt order and measurable antisite disorder, while x-ray absorption near-edge structure identifies and valence states. Magnetometry reveals a ferromagnetic (FM) transition at driven by exchange, followed at lower temperature by a ferrimagneticlike (FiM) regime when the and sublattices are magnetically ordered. Concomitantly, Raman modes exhibit anomalous hardening below and the refined SXRD lattice parameters display clear anomalies at the magnetic transitions, evidencing pronounced magnetoelastic coupling. Spin-polarized density functional theory captures this competition, yielding nearly degenerate FiM and FM solutions ( per 20-atom cell) and indicating that coupling of the rare-earth sublattice to the Ni-O-Mn network sets the energy balance. The ferrimagnetic solution carries local moments of on Ni and on Mn and remains insulating, with a gap of 1.6–1.7 eV. With spin-orbit coupling (SOC), the projected spin moment is strongly reduced (4.93 to 0.3 ), reflecting SOC-driven quenching of the Sm spin polarization, while the gap is nearly unchanged, indicating that the electronic structure is primarily stabilized by Ni/Mn –O hybridization. Our results provide a quantitative framework to disentangle rare-earth -site magnetism from Ni-O-Mn exchange and to rationalize magnetoelastic responses in -site-disordered double perovskites near competing magnetic states.